A supramolecular cocrystal of 2-ammino-5-nitropyridine (ANP) with 2,4-dinitrophenol (DNP) has been successfully grown by the slow evaporation solution growth technique. The crystal structure 2-amino-5-nitropyridine-2,4-dinitrophenol (ANDP) was elucidated single-crystal X-ray diffraction analysis, and it belongs to a monoclinic system centrosymmetric space group P21/n. bulk phase purity homogene...

We investigate whether microscopic cascading of second-order nonlinearities of two molecules in the side-byside configuration can lead to a third-order molecular nonlinear-optical response that exceeds the fundamental limit. We find that for large values of the second hyperpolarizability, the side-by-side configuration has a cascading contribution that lowers the direct contribution. However, w...

A comprehensive theoretical study was carried out on a series of aryldimesityl borane (DMB) derivatives using Density Functional theory. Optimized geometries and electronic parameters like electron affinity, reorganization energy, frontiers molecular contours, polarizability and hyperpolarizability have been calculated by employing B3PW91/6-311++G (d, p) level of theory. Our results show that t...

Calculations of the hyperpolarizability are typically much more difficult to converge with basis set size than the linear polarizability. In order to understand these convergence issues and hence obtain accurate ab initio values, we compare calculations of the static hyperpolarizability of the gas-phase chloroform molecule (CHCl(3)) using three different kinds of basis sets: Gaussian-type orbit...

The Schrödinger equation has the property that when changing the length scale by ~r → ǫ~r and the energy scale by E → E/ǫ, the shape of the wavefunction remains unchanged. The same re-scaling leaves the intrinsic hyperpolarizability (as well as higher-order hyperpolarizabilities) unchanged. As such, the intrinsic hyperpolarizability is the best quantity for comparing molecules since it re-norma...

A polarization-resolved beam deflection technique is used to separate the bound-electronic and molecular rotational components of nonlinear refractive transients of molecular gases. Coherent rotational revivals from N(2), O(2), and two isotopologues of carbon disulfide (CS(2)), are identified in gaseous mixtures. Dephasing rates, rotational and centrifugal distortion constants of each species a...

We present a general approach for the analytic calculation of pure vibrational contributions to the molecular (hyper)polarizabilities at the density functional level of theory. The analytic approach allows us to study large molecules, and we apply the new code to the study of the first dipole hyperpolarizabilities of retinal and related molecules. We investigate the importance of electron corre...

Recent Hyper Rayleigh Scattering measurements report a significant increase of second-order hyperpolarizability upon introduction of positive charges at the pyridyl end groups in trispyridyl octopolar chromophores. We calculated the geometries, linear response, and first-order hyperpolarizabilities of a series of six trispyridyl molecules both in the neutral and protonated forms. The calculatio...

The equilibrium geometry and harmonic frequencies of the 6-methylnicotinic acid, were determined and analyzed at DFT level employing the basis set 6-311+G(d,p). The skeleton of the optimized molecule is non-planar. In general, a good agreement between experimental and calculated normal modes of vibrations has been observed. The molecular electrostatic potential surface has been used along with ...